格式化
氧化还原
X射线光电子能谱
法拉第效率
催化作用
密度泛函理论
化学
离解(化学)
铈
材料科学
纳米花
氧化铈
锡
拉曼光谱
无机化学
化学工程
光化学
电解质
电极
物理化学
计算化学
工程类
物理
光学
冶金
生物化学
作者
Hai Liu,Boyang Li,Zhihui Liu,Zhaohui Liang,Hongyuan Chuai,Hui Wang,Shi Nee Lou,Yaqiong Su,Sheng Zhang,Xinbin Ma
标识
DOI:10.1021/acscatal.2c06135
摘要
Electrocatalytic CO2 reduction has been considered an effective carbon neutrality as well as energy storage strategy integrated with renewable electricity. CO2 conversion to formate is a feasible route using earth-abundant and nontoxic tin-based catalysts. However, they suffer from degradation and thus decrease in formate selectivity during operation. Guided by density functional theory (DFT) calculations, herein, we synthesized CeO2–SnO2 heterostructures by a facile electrospinning method, which exhibited a maximum formate partial current density of ∼500 mA·cm–2 with 87.1% faradaic efficiency and a long-term stability in a flow cell. Proved by in situ attenuated total reflectance infrared absorption spectroscopy (ATR-IRAS) and Raman spectra as well as post-X-ray photoelectron spectroscopy (XPS) analysis, a dynamic CeO2-mediated Sn0/Snδ+ redox cycle mechanism was proposed: oxygen vacancies generated on cerium oxides prompted water dissociation to produce *OH and *H species, where the former oxidize Sn0 into active Snδ+, facilitating the conversion of CO2 to the key intermediate *OCHO with the help of the latter. This work may provide a general strategy to design stable and efficient catalysts for practical CO2 electrolyzers.
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